scholarly journals Analysis of the latitudinal variability of tropospheric ozone in the Arctic using the large number of aircraft and ozonesonde observations in early summer 2008

2016 ◽  
Author(s):  
Gerard Ancellet ◽  
Nikos Daskalakis ◽  
Jean Christophe Raut ◽  
Boris Quennehen ◽  
François Ravetta ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Tropospheric Ozone ◽  
Lower Troposphere ◽  
Early Summer ◽  
Ozone Production ◽  
The Arctic ◽  
Integrated Analysis ◽  
International Polar Year ◽  
Latitude Range ◽  
Vertical Variability

Abstract. The goal of the paper are to: (1) present tropospheric ozone (O3) climatologies in summer 2008 based on a large amount of measurements, during the International Polar Year when the Polar Study using Aircraft, Remote Sensing, Surface Measurements, and Models of Climate Chemistry, Aerosols, and Transport (POLARCAT) campaigns were conducted (2) investigate the processes that determine O3 concentrations in two different regions (Canada and Greenland) that were thoroughly studied using measurements from 3 aircraft and 7 ozonesonde stations. This paper provides an integrated analysis of these observations and the discussion of the latitudinal and vertical variability of tropospheric ozone north of 55° N during this period is performed using a regional model (WFR-Chem). Ozone, CO and potential vorticity (PV) distributions are extracted from the simulation at the measurement locations. The model is able to reproduce the O3 latitudinal and vertical variability but a negative O3 bias of 6–15 ppbv is found in the free troposphere over 4 km, especially over Canada. Ozone average concentrations are of the order of 65 ppbv at altitudes above 4 km both over Canada and Greenland, while they are less than 50 ppbv in the lower troposphere. The relative influence of stratosphere-troposphere exchange (STE) and of ozone production related to the local biomass burning (BB) emissions is discussed using differences between average values of O3, CO and PV for Southern and Northern Canada or Greenland and two vertical ranges in the troposphere: 0–4 km and 4–8 km. For Canada, the model CO distribution and the weak correlation (< 30 %) of O3 and PV suggests that stratosphere-troposphere exchange (STE) is not the major contribution to average tropospheric ozone at latitudes less than 70° N, due to the fact that local biomass burning (BB) emissions were significant during the 2008 summer period. Conversely over Greenland, significant STE is found according to the better O3 versus PV correlation (> 40 %) and the higher 75th PV percentile. A weak negative latitudinal summer ozone gradient −6 to −8 ppbv is found over Canada in the mid troposphere between 4 and 8 km. This is attributed to an efficient O3 photochemical production due to the BB emissions at latitudes less than 65° N, while STE contribution is more homogeneous in the latitude range 55° N to 70° N. A positive ozone latitudinal gradient of 12 ppbv is observed in the same altitude range over Greenland not because of an increasing latitudinal influence of STE, but because of different long range transport from multiple mid-latitude sources (North America, Europe and even Asia for latitudes higher than 77° N).

scholarly journals Analysis of the latitudinal variability of tropospheric ozone in the Arctic using the large number of aircraft and ozonesonde observations in early summer 2008

2016 ◽  
Vol 16 (20) ◽  
pp. 13341-13358 ◽  
Author(s):  
Gerard Ancellet ◽  
Nikos Daskalakis ◽  
Jean Christophe Raut ◽  
David Tarasick ◽  
Jonathan Hair ◽  
...  
Keyword(s):  
Tropospheric Ozone ◽  
Average Concentration ◽  
Early Summer ◽  
Airborne Lidar ◽  
The Arctic ◽  
Integrated Analysis ◽  
Free Troposphere ◽  
International Polar Year ◽  
Latitude Range ◽  
Vertical Variability

Abstract. During the 2008 International Polar Year, the POLARCAT (Polar Study using Aircraft, Remote Sensing, Surface Measurements, and Models of Climate Chemistry, Aerosols, and Transport) campaign, conducted in summer over Greenland and Canada, produced a large number of measurements from three aircraft and seven ozonesonde stations. Here we present an observation-integrated analysis based on three different types of O3 measurements: airborne lidar, airborne UV absorption or chemiluminescence measurement, and intensified electrochemical concentration cell (ECC) ozonesonde profiles. Discussion of the latitudinal and vertical variability of tropospheric ozone north of 55° N during this period is performed with the aid of a regional model (WFR-Chem). The model is able to reproduce the O3 latitudinal and vertical variability but with a negative O3 bias of 6–15 ppbv in the free troposphere above 4 km, especially over Canada. For Canada, large average CO concentrations in the free troposphere above 4 km ( >  130 ppbv) and the weak correlation (<  30 %) of O3 and PV suggest that stratosphere–troposphere exchange (STE) is not the major contributor to average tropospheric ozone at latitudes less than 70° N, due to the fact that local biomass burning (BB) emissions were significant during the 2008 summer period. Conversely, significant STE is found over Greenland according to the better O3 vs. PV correlation ( >  40 %) and the higher values of the 75th PV percentile. It is related to the persistence of cyclonic activity during the summer over Baffin Bay. Using differences between average concentration above Northern and Southern Canada, a weak negative latitudinal summer ozone gradient of −6 to −8 ppbv is found in the mid-troposphere between 4 and 8 km. This is attributed to an efficient O3 photochemical production from BB emissions at latitudes less than 65° N, while the STE contribution is more homogeneous in the latitude range 55–70° N. A positive ozone latitudinal gradient of 12 ppbv is observed in the same altitude range over Greenland not because of an increasing latitudinal influence of STE, but because of different long-range transport from multiple mid-latitude sources (North America, Europe, and even Asia for latitudes higher than 77° N). For the Arctic latitudes (>  80° N), free tropospheric O3 concentrations during summer 2008 are related to a mixture of Asian pollution and stratospheric O3 transport across the tropopause.

scholarly journals Biomass burning influence on high latitude tropospheric ozone and reactive nitrogen in summer 2008: a multi-model analysis based on POLMIP simulations

2014 ◽  
Vol 14 (17) ◽  
pp. 24573-24621 ◽  
Author(s):  
S. R. Arnold ◽  
L. K. Emmons ◽  
S. A. Monks ◽  
K. S. Law ◽  
D. A. Ridley ◽  
...  
Keyword(s):  
Biomass Burning ◽  
High Latitude ◽  
Tropospheric Ozone ◽  
Transport Model ◽  
Chemical Transport ◽  
Ozone Production ◽  
The Arctic ◽  
Vertical Position ◽  
Chemical Transport Model ◽  
Fire Emissions

Abstract. We have evaluated tropospheric ozone enhancement in air dominated by biomass burning emissions at high laititudes (> 50˚ N) in July 2008, using 10 global chemical transport model simulations from the POLMIP multi-model comparison exercise. In model air masses dominated by fire emissions, Δ O3/ΔCO values ranged between 0.039 and 0.196 ppbv ppbv−1 (mean: 0.113 ppbv ppbv−1) in freshly fire-influenced air, and between 0.140 and 0.261 ppbv ppbv−1 (mean: 0.193 ppbv) in more aged fire-influenced air. These values are in broad agreement with the range of observational estimates from the literature. Model ΔPAN/ΔCO enhancement ratios show distinct groupings according to the meteorological data used to drive the models. ECMWF-forced models produce larger ΔPAN/ΔCO values (4.44–6.28 pptv ppbv−1) than GEOS5-forced models (2.02–3.02 pptv ppbv−1), which we show is likely linked to differences efficiency of vertical transport during poleward export from mid-latitude source regions. Simulations of a large plume of biomass burning and anthropogenic emissions exported from Asia towards the Arctic using a Lagrangian chemical transport model show that 4 day net ozone change in the plume is sensitive to differences in plume chemical composition and plume vertical position among the POLMIP models. In particular, Arctic ozone evolution in the plume is highly sensitive to initial concentrations of PAN, as well as oxygenated VOCs (acetone, acetaldehyde), due to their role in producing the peroxyacetyl radical PAN precursor. Vertical displacement is also important due to its effects on the stability of PAN, and subsequent effect on NOx abundance. In plumes where net ozone production is limited, we find that the lifetime of ozone in the plume is sensitive to hydrogen peroxide loading, due to the production of HO2 from peroxide photolysis, and the key role of HO2 + O3 in controlling ozone loss. Overall, our results suggest that emissions from biomass burning lead to large-scale photochemical enhancement in high latitude tropospheric ozone during summer.

scholarly journals Biomass burning influence on high-latitude tropospheric ozone and reactive nitrogen in summer 2008: a multi-model analysis based on POLMIP simulations

2015 ◽  
Vol 15 (11) ◽  
pp. 6047-6068 ◽  
Author(s):  
S. R. Arnold ◽  
L. K. Emmons ◽  
S. A. Monks ◽  
K. S. Law ◽  
D. A. Ridley ◽  
...  
Keyword(s):  
Biomass Burning ◽  
High Latitude ◽  
Tropospheric Ozone ◽  
Transport Model ◽  
Chemical Transport ◽  
Ozone Production ◽  
The Arctic ◽  
Vertical Position ◽  
Chemical Transport Model ◽  
Fire Emissions

Abstract. We have evaluated tropospheric ozone enhancement in air dominated by biomass burning emissions at high latitudes (> 50° N) in July 2008, using 10 global chemical transport model simulations from the POLMIP multi-model comparison exercise. In model air masses dominated by fire emissions, ΔO3/ΔCO values ranged between 0.039 and 0.196 ppbv ppbv−1 (mean: 0.113 ppbv ppbv−1) in freshly fire-influenced air, and between 0.140 and 0.261 ppbv ppbv−1 (mean: 0.193 ppbv) in more aged fire-influenced air. These values are in broad agreement with the range of observational estimates from the literature. Model ΔPAN/ΔCO enhancement ratios show distinct groupings according to the meteorological data used to drive the models. ECMWF-forced models produce larger ΔPAN/ΔCO values (4.47 to 7.00 pptv ppbv−1) than GEOS5-forced models (1.87 to 3.28 pptv ppbv−1), which we show is likely linked to differences in efficiency of vertical transport during poleward export from mid-latitude source regions. Simulations of a large plume of biomass burning and anthropogenic emissions exported from towards the Arctic using a Lagrangian chemical transport model show that 4-day net ozone change in the plume is sensitive to differences in plume chemical composition and plume vertical position among the POLMIP models. In particular, Arctic ozone evolution in the plume is highly sensitive to initial concentrations of PAN, as well as oxygenated VOCs (acetone, acetaldehyde), due to their role in producing the peroxyacetyl radical PAN precursor. Vertical displacement is also important due to its effects on the stability of PAN, and subsequent effect on NOx abundance. In plumes where net ozone production is limited, we find that the lifetime of ozone in the plume is sensitive to hydrogen peroxide loading, due to the production of HOx from peroxide photolysis, and the key role of HO2 + O3 in controlling ozone loss. Overall, our results suggest that emissions from biomass burning lead to large-scale photochemical enhancement in high-latitude tropospheric ozone during summer.

scholarly journals Tropospheric ozone over Equatorial Africa: regional aspects from the MOZAIC data

2004 ◽  
Vol 4 (3) ◽  
pp. 3285-3332 ◽  
Author(s):  
B. Sauvage ◽  
V. Thouret ◽  
J.-P. Cammas ◽  
F. Gheusi ◽  
G. Athier ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Tropospheric Ozone ◽  
Central Africa ◽  
Lower Troposphere ◽  
Boreal Summer ◽  
Boreal Winter ◽  
Vertical Profiles ◽  
Middle Troposphere ◽  
Ozone Distribution ◽  
Equatorial Africa

Abstract. We analyze MOZAIC ozone observations recorded over Equatorial Africa, from April 1997 to March 2003 to give the first ozone climatology of this region. The monthly mean vertical profiles have been systematically analyzed with monthly mean ECMWF data using a Lagrangian-model (LAGRANTO). We assess the roles played by the dynamical features of Equatorial Africa and the intense biomass burning sources within the region in defining the ozone distribution. The lower troposphere exhibits layers of enhanced ozone during the biomass burning season in each hemisphere (boreal winter in the northern tropics and boreal summer in the southern tropics). The monthly mean vertical profiles of ozone are clearly influenced by the local dynamical situation. Over the Gulf of Guinea during boreal winter, the ozone profile is characterized by systematically high ozone below 650 hPa. This is due to the high stability caused by the Harmattan winds in the lower troposphere and the blocking Saharan anticyclone in the middle troposphere that prevents any efficient vertical mixing. In contrast, Central African enhancements are not only found in the lower troposphere but throughout the troposphere. The boreal summer ozone maximum in the lower troposphere of Central Africa continues up to November in the middle troposphere due to the influx of air masses laden with biomass burning products from Brazil and Southern Africa. Despite its southern latitude, Central Africa during the boreal winter is also under the influence of the northern tropical fires. This phenomenon is known as the "ozone paradox". However, the tropospheric ozone columns calculated from the MOZAIC data give evidence that the Tropical Tropospheric Ozone Column (TTOC) maximum over Africa swings from West Africa in DJF to Central Africa in JJA. This contrasts with studies based on TOMS satellite data. A rough assessment of the regional ozone budget shows that the northern tropics fires in boreal winter might contribute up to 20% of the global photochemical ozone production. This study gives the first detailed picture of the ozone distribution over Equatorial Africa that should be used to validate both global models over this region and future satellite products.

scholarly journals Sources of Springtime Surface Black Carbon in the Arctic: An Adjoint Analysis

2017 ◽  
Author(s):  
Ling Qi ◽  
Qinbin Li ◽  
Daven K. Henze ◽  
Hsien-Liang Tseng ◽  
Cenlin He
Keyword(s):  
Natural Gas ◽  
Black Carbon ◽  
Biomass Burning ◽  
Transport Model ◽  
Lower Troposphere ◽  
Anthropogenic Sources ◽  
The Arctic ◽  
Anthropogenic Source ◽  
Gas Flaring ◽  
Arctic Front

Abstract. We quantify source contributions to springtime (April 2008) surface black carbon (BC) in the Arctic by interpreting surface observations of BC at five receptor sites (Denali, Barrow, Alert, Zeppelin, and Summit) using a global chemical transport model (GEOS-Chem) and its adjoint. Contributions to BC at Barrow, Alert, and Zeppelin are dominated by Asian anthropogenic sources (40–43 %) before April 18 and by Siberian open biomass burning emissions (29–41 %) afterward. In contrast, Summit, a mostly free tropospheric site, has predominantly an Asian anthropogenic source contribution (24–68 %, with an average of 45 %). We compute the adjoint sensitivity of BC concentrations at the five sites during a pollution episode (April 20–25) to global emissions from March 1 to April 25. The associated contributions are the combined results of these sensitivities and BC emissions. Local and regional anthropogenic sources in Alaska are the largest anthropogenic sources of BC at Denali (63 %), and natural gas flaring emissions in the Western Extreme North of Russia (WENR) are the largest anthropogenic sources of BC at Zeppelin (26 %) and Alert (13 %). We find that long-range transport of emissions from Beijing-Tianjin-Hebei (also known as Jing-Jin-Ji), the biggest urbanized region in Northern China, contribute significantly (~ 10 %) to surface BC across the Arctic. On average it takes ~ 12 days for Asian anthropogenic emissions and Siberian biomass burning emissions to reach Arctic lower troposphere, supporting earlier studies. Natural gas flaring emissions from the WENR reach Zeppelin in about a week. We find that episodic, direct transport events dominate BC at Denali (87 %), a site outside the Arctic front, a strong transport barrier. The relative contribution of direct transport to surface BC within the Arctic front is much smaller (~ 50 % at Barrow and Zeppelin and ~ 10 % at Alert). The large contributions from Asian anthropogenic sources are predominately in the form of ‘chronic’ pollution (~ 40 % at Barrow and 65 % at Alert and 57 % at Zeppelin) on 1–2 month timescales. As such, it is likely that previous studies using 5- or 10-day trajectory analyses strongly underestimated the contribution from Asia to surface BC in the Arctic. Both finer temporal resolution of biomass burning emissions and accounting for the Wegener-Bergeron-Findeisen (WBF) process in wet scavenging improve the source attribution estimates.

scholarly journals Stratospheric impact on the Northern Hemisphere winter and spring ozone interannual variability in the troposphere

2019 ◽  
Author(s):  
Junhua Liu ◽  
Jose M. Rodriguez ◽  
Luke D. Oman ◽  
Anne R. Douglass ◽  
Mark A. Olsen ◽  
...  
Keyword(s):  
North America ◽  
Tropospheric Ozone ◽  
Interannual Variation ◽  
Stratospheric Ozone ◽  
Lower Troposphere ◽  
The Arctic ◽  
Vertical Extent ◽  
Pinatubo Eruption ◽  
Tropospheric O3 ◽  
The Impact

Abstract. In this study we use O3 and stratospheric O3 tracer simulations from the high-resolution Goddard Earth Observing System, Version 5 (GEOS-5) Replay run (MERRA-2 GMI at 0.5° model resolution ~ 50 km) and observations from ozonesondes to investigate the interannual variation and vertical extent of the stratospheric ozone impact on tropospheric ozone. Our work focuses on the winter and spring seasons over North America and Europe. The model reproduces the observed interannual variation of tropospheric O3, except for the Pinatubo period from 1991 to 1995 over the region of North America. Ozonesonde data show a negative ozone anomaly in 1992–1994 following the Pinatubo eruption, with recovery thereafter. The simulated anomaly is only half the magnitude of that observed. Our analysis suggests that the simulated Stratosphere-troposphere exchange (STE) flux deduced from the analysis might be too strong over the North American (50° N–70° N) region after the Mt. Pinatubo eruption in the early 1990s, masking the impact of lower stratospheric O3 concentration on tropospheric O3. European ozonesonde measurements show a similar but weaker O3 depletion after the Mt. Pinatubo eruption, which is fully reproduced by the model. Analysis based on a stratospheric O3 tracer (StratO3) identifies differences in strength and vertical extent of stratospheric ozone influence on the tropospheric ozone interannual variation (IAV) between North America and Europe. Over North America, the StratO3 IAV has a significant impact on tropospheric O3 from the upper to lower troposphere and explains about 60 % and 66 % of simulated O3 IAV at 400 hPa, ~ 11 % and 34 % at 700 hPa in winter and spring respectively. Over Europe, the influence is limited to the middle to upper troposphere, and becomes much smaller at 700 hPa. The stronger and deeper stratospheric contributions in the tropospheric O3 IAV over North America shown by the model is likely related to ozonesondes' being closer to the polar vortex in winter with lower geopotential height, lower tropopause height, and stronger coupling to the Arctic Oscillation in the lower troposphere (LT) than over Europe.

scholarly journals Reactive nitrogen, ozone and ozone production in the Arctic troposphere and the impact of stratosphere-troposphere exchange

2011 ◽  
Vol 11 (24) ◽  
pp. 13181-13199 ◽  
Author(s):  
Q. Liang ◽  
J. M. Rodriguez ◽  
A. R. Douglass ◽  
J. H. Crawford ◽  
J. R. Olson ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Stratospheric Ozone ◽  
Arctic Region ◽  
Ozone Production ◽  
The Arctic ◽  
Subsequent Formation ◽  
Air Masses ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
The Impact

Abstract. We use aircraft observations obtained during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission to examine the distributions and source attributions of O3 and NOy in the Arctic and sub-Arctic region. Using a number of marker tracers, we distinguish various air masses from the background troposphere and examine their contributions to NOx, O3, and O3 production in the Arctic troposphere. The background Arctic troposphere has a mean O3 of ~60 ppbv and NOx of ~25 pptv throughout spring and summer with CO decreasing from ~145 ppbv in spring to ~100 ppbv in summer. These observed mixing ratios are not notably different from the values measured during the 1988 ABLE-3A and the 2002 TOPSE field campaigns despite the significant changes in emissions and stratospheric ozone layer in the past two decades that influence Arctic tropospheric composition. Air masses associated with stratosphere-troposphere exchange are present throughout the mid and upper troposphere during spring and summer. These air masses, with mean O3 concentrations of 140–160 ppbv, are significant direct sources of O3 in the Arctic troposphere. In addition, air of stratospheric origin displays net O3 formation in the Arctic due to its sustainable, high NOx (75 pptv in spring and 110 pptv in summer) and NOy (~800 pptv in spring and ~1100 pptv in summer). The air masses influenced by the stratosphere sampled during ARCTAS-B also show conversion of HNO3 to PAN. This active production of PAN is the result of increased degradation of ethane in the stratosphere-troposphere mixed air mass to form CH3CHO, followed by subsequent formation of PAN under high NOx conditions. These findings imply that an adequate representation of stratospheric NOy input, in addition to stratospheric O3 influx, is essential to accurately simulate tropospheric Arctic O3, NOx and PAN in chemistry transport models. Plumes influenced by recent anthropogenic and biomass burning emissions observed during ARCTAS show highly elevated levels of hydrocarbons and NOy (mostly in the form of NOx and PAN), but do not contain O3 higher than that in the Arctic tropospheric background except some aged biomass burning plumes sampled during spring. Convection and/or lightning influences are negligible sources of O3 in the Arctic troposphere but can have significant impacts in the upper troposphere in the continental sub-Arctic during summer.

scholarly journals Sources of springtime surface black carbon in the Arctic: an adjoint analysis for April 2008

2017 ◽  
Vol 17 (15) ◽  
pp. 9697-9716 ◽  
Author(s):  
Ling Qi ◽  
Qinbin Li ◽  
Daven K. Henze ◽  
Hsien-Liang Tseng ◽  
Cenlin He
Keyword(s):  
Natural Gas ◽  
Black Carbon ◽  
Biomass Burning ◽  
Transport Model ◽  
Lower Troposphere ◽  
Anthropogenic Sources ◽  
The Arctic ◽  
Anthropogenic Source ◽  
Chemical Transport Model ◽  
Gas Flaring

Abstract. We quantify source contributions to springtime (April 2008) surface black carbon (BC) in the Arctic by interpreting surface observations of BC at five receptor sites (Denali, Barrow, Alert, Zeppelin, and Summit) using a global chemical transport model (GEOS-Chem) and its adjoint. Contributions to BC at Barrow, Alert, and Zeppelin are dominated by Asian anthropogenic sources (40–43 %) before 18 April and by Siberian open biomass burning emissions (29–41 %) afterward. In contrast, Summit, a mostly free tropospheric site, has predominantly an Asian anthropogenic source contribution (24–68 %, with an average of 45 %). We compute the adjoint sensitivity of BC concentrations at the five sites during a pollution episode (20–25 April) to global emissions from 1 March to 25 April. The associated contributions are the combined results of these sensitivities and BC emissions. Local and regional anthropogenic sources in Alaska are the largest anthropogenic sources of BC at Denali (63 % of total anthropogenic contributions), and natural gas flaring emissions in the western extreme north of Russia (WENR) are the largest anthropogenic sources of BC at Zeppelin (26 %) and Alert (13 %). We find that long-range transport of emissions from Beijing–Tianjin–Hebei (also known as Jing–Jin–Ji), the biggest urbanized region in northern China, contribute significantly (∼ 10 %) to surface BC across the Arctic. On average, it takes ∼ 12 days for Asian anthropogenic emissions and Siberian biomass burning emissions to reach the Arctic lower troposphere, supporting earlier studies. Natural gas flaring emissions from the WENR reach Zeppelin in about a week. We find that episodic transport events dominate BC at Denali (87 %), a site outside the Arctic front, which is a strong transport barrier. The relative contribution of these events to surface BC within the polar dome is much smaller (∼ 50 % at Barrow and Zeppelin and ∼ 10 % at Alert). The large contributions from Asian anthropogenic sources are predominately in the form of chronic pollution (∼ 40 % at Barrow, 65 % at Alert, and 57 % at Zeppelin) on about a 1-month timescale. As such, it is likely that previous studies using 5- or 10-day trajectory analyses strongly underestimated the contribution from Asia to surface BC in the Arctic.

scholarly journals Remote sensed and in situ constraints on processes affecting tropical tropospheric ozone

2006 ◽  
Vol 6 (6) ◽  
pp. 11465-11520 ◽  
Author(s):  
B. Sauvage ◽  
R. V. Martin ◽  
A. van Donkelaar ◽  
X. Liu ◽  
K. Chance ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Tropospheric Ozone ◽  
Transport Model ◽  
Lower Troposphere ◽  
In Situ Measurements ◽  
Top Down ◽  
Upper Troposphere ◽  
In Situ Observations ◽  
Tropospheric O3

Abstract. We use a global chemical transport model (GEOS-Chem) to evaluate the consistency of satellite measurements of lightning flashes and ozone precursors with in situ measurements of tropical tropospheric ozone. The measurements are tropospheric O3, NO2, and HCHO columns from the GOME satellite instrument, lightning flashes from the OTD and LIS instruments, profiles of O3, CO, and relative humidity from the MOZAIC aircraft program, and profiles of O3 from the SHADOZ ozonesonde network. We interpret these multiple data sources with our model to better understand what controls tropical tropospheric ozone. Tropical tropospheric ozone is mainly affected by lightning and convection in the upper troposphere and by surface emissions in the lower troposphere. Scaling the spatial distribution of lightning in the model to the observed flash counts improves the simulation of O3 in the upper troposphere by 5–20 ppbv versus in situ observations and by 1–4 Dobson Units versus GOME retrievals of tropospheric O3 columns. A lightning source strength of 5±2 Tg N/yr best represents in situ observations from aircraft and ozonesonde. Tropospheric NO2 and HCHO columns from GOME are applied to provide top-down constraints on emission inventories of NOx (biomass burning and soils) and VOCs (biomass burning). The top-down biomass burning inventory is larger by a factor of 2 for HCHO and alkenes, and by 2.6 for NOx over northern equatorial Africa. These emissions increase lower tropospheric O3 by 5–20 ppbv, improving the simulation versus aircraft observations, and by 4 Dobson Units versus GOME observations of tropospheric O3 columns. Emission factors in the a posteriori inventory are more consistent with a recent compilation from in situ measurements. The ozone simulation using two different dynamical schemes (GEOS-3 and GEOS-4) is evaluated versus observations; GEOS-4 better represents O3 observations by 5–15 ppbv due to enhanced convective detrainment in the upper troposphere. Heterogeneous uptake of HNO3 on aerosols reduces simulated O3 by 5–7 ppbv, reducing a model bias versus in situ observations over and downwind of deserts. Exclusion of HO2 uptake on aerosols improves O3 by 5 ppbv in biomass burning regions.

scholarly journals Reactive nitrogen, ozone and ozone production in the Arctic troposphere and the impact of stratosphere-troposphere exchange

2011 ◽  
Vol 11 (4) ◽  
pp. 10721-10767 ◽  
Author(s):  
Q. Liang ◽  
J. M. Rodriguez ◽  
A. R. Douglass ◽  
J. H. Crawford ◽  
E. Apel ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Arctic Region ◽  
Tropospheric Chemistry ◽  
Ozone Production ◽  
The Arctic ◽  
Source Attribution ◽  
Air Masses ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
The Impact

Abstract. We analyze the aircraft observations obtained during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellite (ARCTAS) mission together with the GEOS-5 CO simulation to examine O3 and NOy in the Arctic and sub-Arctic region and their source attribution. Using a number of marker tracers and their probability density distributions, we distinguish various air masses from the background troposphere and examine their contribution to NOx, O3, and O3 production in the Arctic troposphere. The background Arctic troposphere has mean O3 of ~60 ppbv and NOx of ~25 pptv throughout spring and summer with CO decreases from ~145 ppbv in spring to ~100 ppbv in summer. These observed CO, NOx and O3 mixing ratios are not notably different from the values measured during the 1988 ABLE-3A and the 2002 TOPSE field campaigns despite the significant changes in the past two decades in processes that could have changed the Arctic tropospheric composition. Air masses associated with stratosphere-troposphere exchange are present throughout the mid and upper troposphere during spring and summer. These air masses with mean O3 concentration of 140–160 ppbv are the most important direct sources of O3 in the Arctic troposphere. In addition, air of stratospheric origin is the only notable driver of net O3 formation in the Arctic due to its sustainable high NOx (75 pptv in spring and 110 pptv in summer) and NOy (~800 pptv in spring and ~1100 pptv in summer) levels. The ARCTAS measurements present observational evidence suggesting significant conversion of nitrogen from HNO3 to NOx and then to PAN (a net formation of ~120 pptv PAN) in summer when air of stratospheric origin is mixed with tropospheric background during stratosphere-to-troposphere transport. These findings imply that an adequate representation of stratospheric O3 and NOy input are essential in accurately simulating O3 and NOx photochemistry as well as the atmospheric budget of PAN in tropospheric chemistry transport models of the Arctic. Anthropogenic and biomass burning pollution plumes observed during ARCTAS show highly elevated hydrocarbons and NOy (mostly in the form of NOx and PAN), but do not contribute significantly to O3 in the Arctic troposphere except in some of the aged biomass burning plumes sampled during spring. Convection and/or lightning influences are negligible sources of O3 in the Arctic troposphere but can have significant impacts in the upper troposphere in the continental sub-Arctic during summer.

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